Synthesis and Characterization of Magnesium Vanadates as Potential Magnesium-Ion Cathode Materials through an Ab Initio Guided Carbothermal Reduction Approach**

Lee, Jeongjae; Dey, Sunita; Dutton, Siân E.; Grey, Clare P.

doi:10.1002/anie.202112688

Synthesis and Characterization of Magnesium Vanadates as Potential Magnesium-Ion Cathode Materials through an Ab Initio Guided Carbothermal Reduction Approach**

Journal Article · Wed Dec 01 00:00:00 EST 2021 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.202112688· OSTI ID:1981385

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University of Cambridge (United Kingdom)

Many technologically relevant materials for advanced energy storage and catalysis feature reduced transition-metal (TM) oxides that are often nontrivial to prepare because of the need to control the reducing nature of the atmosphere in which they are synthesized. In this report, we show that an ab initio predictive synthesis strategy can be used to produce multi-gram-scale products of various MgV_xO_y-type phases (δ-MgV₂O₅, spinel MgV₂O₄, and MgVO₃) containing V³⁺ or V⁴⁺ relevant for Mg-ion battery cathodes. Characterization of these phases using ²⁵Mg solid-state NMR spectroscopy illustrates the potential of ²⁵Mg NMR for studying reversible magnesiation and local charge distributions. Rotor-assisted population transfer (RAPT) is used as a much-needed signal-to-noise enhancement technique. The ab initio guided synthesis method is seen as a step forward towards a predictive synthesis strategy for targeting specific complex TM oxides with variable oxidation states of technological importance.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN); University of Cambridge (United Kingdom)

Sponsoring Organization:: European Union's Horizon 2020; USDOE; USDOE Office of Science (SC)

Grant/Contract Number:: SC0012704

OSTI ID:: 1981385

Alternate ID(s):: OSTI ID: 1839294
OSTI ID: 23116404

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 8 Vol. 61; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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